Reducing Carbonaceous Salts for Facile Fabrication of Monolayer Graphene

Abstract Novel methods and mechanisms for graphene fabrication are of great importance in the development of materials science. Herein, a facile method to directly convert carbonaceous salts into high‐quality freestanding graphene via a simple one‐step redox reaction, is reported. The redox couple can be a combination of sodium borohydride (reductant) and sodium carbonate (oxidant), which can readily react with each other when evenly mixed/calcined and yield gram‐scale, high‐quality, contamination‐free, micron‐sized, freestanding graphene. More importantly, this method is applicable to a variety of input reductants and oxidants that are low cost and easily accessible. An in‐depth investigation reveals that the carbonaceous oxidants can not only provide reduced carbon mass for graphene formation but also act as a self‐template to guide the polymerization of carbon atoms following the pattern of the monolayer, six‐carbon rings. In addition, the direct formation of graphene exhibits theoretically lower energy barriers than that of other allotropes such as fullerene and carbon nanotube. This facile, low‐cost, scalable, and applicable method for mass production of high‐quality graphene is expected to revolutionize graphene fabrication technology and boost its practical application to the industry level.